ARTICLES
PUBLISHED ONLINE: 24 APRIL 2011 | DOI: 10.1038/NPHYS1983
Controlled near-field enhanced electron
acceleration from dielectric nanospheres with
intense few-cycle laser fields
Sergey Zherebtsov
1 †
, Thomas Fennel
2
*
†
, Jürgen Plenge
3†
, Egill Antonsson
3
, Irina Znakovskaya
1
,
Adrian Wirth
1
, Oliver Herrwerth
1
, Frederik Süßmann
1
, Christian Peltz
2
, Izhar Ahmad
1
,
Sergei A. Trushin
1
, Vladimir Pervak
4
, Stefan Karsch
1,4
, Marc J. J. Vrakking
5,6
, Burkhard Langer
3
,
Christina Graf
3
, Mark I. Stockman
1,7
, Ferenc Krausz
1,4
, Eckart Rühl
3
*
and Matthias F. Kling
1,8,9
*
Collective electron motion in condensed matter typically unfolds on a sub-femtosecond timescale. The well-defined electric
field evolution of intense, phase-stable few-cycle laser pulses provides an ideal tool for controlling this motion. The resulting
manipulation of local electric fields at nanometre spatial and attosecond temporal scales offers unique spatio-temporal control
of ultrafast nonlinear processes at the nanoscale, with important implications for the advancement of nanoelectronics. Here we
demonstrate the attosecond control of the collective electron motion and directional emission from isolated dielectric (SiO
2
)
nanoparticles with phase-stabilized few-cycle laser fields. A novel acceleration mechanism leading to the ejection of highly
energetic electrons is identified by the comparison of the results to quasi-classical model calculations. The observed lightwave
control in nanosized dielectrics has important implications for other material groups, including semiconductors and metals.
T
he interaction of nanostructured materials with few-cycle
laser light is at present attracting significant attention
1–3
.
This interest is driven both by the quest for fundamental
insight into the real-time many-electron dynamics and a wide range
of applications, including ultrafast computation and information
storage on the nanoscale
4
, the generation of extreme ultraviolet
(XUV) frequency combs
3
, and plasmon-enhanced photoprocesses
in femtosecond photochemistry, light detection, and solar energy
conversion
5
. Access to the attosecond dynamics of nanostructured
materials under laser light at optical frequencies became feasible
with the availability of waveform-controlled near single-cycle
optical fields
6
and XUV light pulses as short as 80 attoseconds
7,8
.
Such light fields have made it possible to study tunnelling
of electrons in atomic ionization
9
, valence electron motion in
atoms
10
, attosecond photoemission dynamics in solids
11
, and may
serve to monitor nanolocalized plasmonic fields with attosecond
temporal resolution
12
.
The key to applications of nanosystems in the ultrafast regime is
the control of nanoscopic electric fields on sub-cycle timescales
12
.
A powerful tool to steer electron dynamics on sub-femtosecond
timescales is the use of phase-controlled few-cycle laser pulses
in the visible
13
, where the electric field evolution is given by
E (t ) = E
0
(t )cos(ωt + ϕ), where E
0
(t ) is the amplitude envelope,
ω the angular frequency of the carrier wave, and ϕ the carrier-
envelope phase (CEP). Waveform-controlled laser fields have been
1
Max Planck Institute of Quantum Optics, Hans-Kopfermann-Str. 1, 85748 Garching, Germany,
2
Institute of Physics, University of Rostock,
Universitätsplatz 3, 18051 Rostock, Germany,
3
Physical Chemistry, Freie Universität Berlin, Takustr. 3, 14195 Berlin, Germany,
4
Physics Department,
Ludwig-Maximilian University, Am Coulombwall 1, 85748 Garching, Germany,
5
Max-Born-Institut, Max-Born Strasse 2A, D-12489 Berlin, Germany,
6
FOM
Institute for Atomic and Molecular Physics, Science Park 113, 1098 XG Amsterdam, The Netherlands,
7
Department of Physics and Astronomy, Georgia
State University, Atlanta, Georgia 30303, USA,
8
J.R. Macdonald Laboratory, Department of Physics, Kansas State University, Manhattan, Kansas 66506,
USA,
9
King Abdullah Institute for Nanotechnology, King Saud University, Riyadh 11451, Saudi Arabia.
†
These authors contributed equally to this work.
*e-mail: thomas.fennel@uni-rostock.de; ruehl@chemie.fu-berlin.de; matthias.kling@mpq.mpg.de.
previously used to control the electron emission from atoms
14
and
electron localization in molecules
15
. One of the most promising
routes to the realization of electronics operating at light wave
frequencies
8
arises from applying such waveform-controlled few-
cycle light fields to nanoscale systems
16–18
.
Recent theoretical work predicts efficient phase control of
surface-plasmon driven electron emission from metallic nanofilms,
where electrons are accelerated by the locally enhanced evanescent
field of laser-induced surface-plasmons
18,19
. Also recollision of elec-
trons in strong laser fields was shown to be important for nanosys-
tems, for example for high-harmonic generation in clusters
20
and
the fragmentation dynamics of C
60
(ref. 21). High-energy electron
emission observed recently in medium sized Ag clusters was as-
cribed to a rescattering process, where electrons are driven through
the cluster by the plasmon-enhanced polarization field
22
. The
present work focuses on dielectric nanoparticles in the gas phase
and reports a novel phase-sensitive acceleration mechanism relying
on electron backscattering from the surface of the nanoparticles
in the presence of a dynamical near field. Dielectric nanoparticles
were chosen as their spectral response is wide allowing the effec-
tive use of the full bandwidth of ultrashort pulses. Furthermore,
the larger work function makes it possible to realize tunnelling
ionization conditions with relatively low ionization yields up to
high intensities, enabling the probing of the dielectric response
with only limited interaction between liberated carriers. By imaging
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